直接碳氢化合物SOFC阳极功能层的制备及性能研究
发布时间：2018-08-29 14:35
【摘要】：固体氧化物燃料电池(SOFC)作为一种高效、清洁的能量转换装置而倍受关注。然而,传统镍基阳极在碳氢化合物燃料的直接运行过程存在严重的积碳问题,成为制约其应用的瓶颈。本文针对镍基阳极的积碳难题,采用热分解法制备镍铁功能层,研究铁的掺杂对功能层的相结构、抗积碳能力及单电池性能的影响；并在此基础上,系统考察了热分解温度、热分解时间、螯合剂种类与添加量以及掺杂元素等因素对Ni0.75Fe0.25功能层抗积碳性能的影响；结合相结构的分析,探讨功能层的相结构与抗积碳性能的相关性规律。首先,对镍铁功能层的相结构、抗积碳性能及单电池性能的研究表明：铁的掺杂能够改善镍的抗积碳性能,Ni0.75Fe0.25功能层的抗积碳性能最好。在650℃甲烷燃料运行下,具有Ni0.75Fe0.25功能层的单电池最大功率密度为326 mW·cm-2,高于其他成分的镍铁功能层制作的单电池；并且该单电池具有最佳的稳定性(运行260分钟后其电压仅衰减9%)。其次,对不同热分解温度和时间制备的Ni0.75Fe0.25功能层的相结构、抗积碳性能及单电池性能的研究表明：705℃1小时制备的Ni0.75Fe0.25功能层的抗积碳性能优于675和735℃1小时制备的功能层；在650℃甲烷燃料运行下,具有705℃制备的Ni0.75Fe0.25功能层的单电池的功率密度和稳定性均高于具有其他温度制备的功能层的单电池。第一性原理计算结果表明,该功能层的FeNi3相各晶面具有最低的表面能,从而改善其抗积碳性能。对705℃下不同热分解时间制备的功能层的研究表明,热分解8小时制得的功能层抗积碳能力最佳,此结果也通过第一性原理计算获得验证。添加不同螯合剂(柠檬酸、乙醇酸和D-葡萄糖酸)制备的Ni0.75Fe0.25功能层,其晶相均为FeNi3相。含D-葡萄糖酸的功能层具有最佳的抗积碳能力；具有该功能层的单电池在650℃甲烷燃料中最大功率达289 mW·cm-2,以600 mA·cm-2的电流密度下运行540分钟后电压仍保持初始电压的61%,高于未添加螯合剂的功能层制作的单电池(53%)。添加不同含量柠檬酸(CA)的功能层中,添加金属离子摩尔量1.5倍的柠檬酸(CA1.5)制备的功能层其各晶面的表面能最低且晶粒尺寸最大,因此具有最佳的抗积碳性能；具有CA1.5功能层的单电池在650℃甲烷中运行540分钟后依然保持74%的电压。此外,本文还研究了Co掺杂对Ni0.75Fe0.25功能层的相结构和抗积碳性能的影响。结果表明：三元功能层的物相为类似FeNi3的尖晶石立方结构；在三元功能层中,(Ni0.75Fe0.25)0.6Co0.4的抗积碳性能最好,此结果也通过第一性原理计算获得了验证。
[Abstract]:Solid oxide fuel cell (SOFC) (SOFC) has attracted much attention as an efficient and clean energy conversion device. However, there is a serious problem of carbon deposition in the direct operation of traditional nickel based anodes in hydrocarbon fuels, which has become the bottleneck of its application. In order to solve the problem of carbon deposition of nickel based anode, the functional layer of nickel iron was prepared by thermal decomposition method. The effect of iron doping on the phase structure, carbon deposition resistance and single cell performance of the functional layer was studied, and the thermal decomposition temperature was investigated systematically. The effects of thermal decomposition time, chelating agent type and amount of chelating agent and doping elements on the anti-carbon deposition performance of Ni0.75Fe0.25 functional layer were discussed, and the correlation between the phase structure and the anti-carbon deposition property of functional layer was discussed by the analysis of phase structure. Firstly, the phase structure, carbon deposition resistance and single cell performance of Ni-Fe functional layer are studied. The results show that Fe doping can improve the carbon deposition performance of Ni 0.75Fe 0.25 functional layer. The maximum power density of the single cell with Ni0.75Fe0.25 functional layer is 326 mW cm-2, higher than that of Ni-Fe functional layer at 650 鈩，
本文编号：2211498
[Abstract]:Solid oxide fuel cell (SOFC) (SOFC) has attracted much attention as an efficient and clean energy conversion device. However, there is a serious problem of carbon deposition in the direct operation of traditional nickel based anodes in hydrocarbon fuels, which has become the bottleneck of its application. In order to solve the problem of carbon deposition of nickel based anode, the functional layer of nickel iron was prepared by thermal decomposition method. The effect of iron doping on the phase structure, carbon deposition resistance and single cell performance of the functional layer was studied, and the thermal decomposition temperature was investigated systematically. The effects of thermal decomposition time, chelating agent type and amount of chelating agent and doping elements on the anti-carbon deposition performance of Ni0.75Fe0.25 functional layer were discussed, and the correlation between the phase structure and the anti-carbon deposition property of functional layer was discussed by the analysis of phase structure. Firstly, the phase structure, carbon deposition resistance and single cell performance of Ni-Fe functional layer are studied. The results show that Fe doping can improve the carbon deposition performance of Ni 0.75Fe 0.25 functional layer. The maximum power density of the single cell with Ni0.75Fe0.25 functional layer is 326 mW cm-2, higher than that of Ni-Fe functional layer at 650 鈩，
本文编号：2211498
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